The development of efficient, earth-abundant electrocatalysts for the oxygen evolution reaction (OER) is of great importance to solar fuel production, because the OER is the half reaction that limits the overall efficency.1-3 Developing catalysts for the OER is especially challenging because the oxidation of water to oxygen occurs through a complex four-electron/four-proton transfer4 and many materials require a significant overpotential to drive the catalysis.5 Traditionally, the best catalysts for the OER have been composed of the noble metals Ru and Ir.6-8 However, since the discovery that iron impurities can improve the OER activity of nickel oxide electrocatalysts,9,10 nickel-iron oxyhydroxides (Ni1-xFexOOH), specifically the layered double hydroxide (LDH) structure of Ni1-xFexOOH, have emerged as promising non-precious metal OER electrocatalysts in alkaline media and can rival the performance of iridium oxides.11-30 